Homogeneous polymer-ionic solvate electrolyte with weak dipole-dipole interaction enabling long cycling pouch lithium metal battery

Likun Chen, Tian Gu, Jinshuo Mi, Yuhang Li, Ke Yang, Jiabin Ma, Xufei An, Yuyuan Jiang, Danfeng Zhang, Xing Cheng, Shaoke Guo, Zhuo Han, Tingzheng Hou, Yidan Cao, Ming Liu (), Wei Lv (), Yan-Bing He () and Feiyu Kang ()
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Likun Chen: Tsinghua Shenzhen International Graduate School, Tsinghua University
Tian Gu: Tsinghua Shenzhen International Graduate School, Tsinghua University
Jinshuo Mi: Tsinghua Shenzhen International Graduate School, Tsinghua University
Yuhang Li: Tsinghua Shenzhen International Graduate School, Tsinghua University
Ke Yang: Tsinghua Shenzhen International Graduate School, Tsinghua University
Jiabin Ma: Tsinghua Shenzhen International Graduate School, Tsinghua University
Xufei An: Tsinghua Shenzhen International Graduate School, Tsinghua University
Yuyuan Jiang: Tsinghua Shenzhen International Graduate School, Tsinghua University
Danfeng Zhang: Tsinghua Shenzhen International Graduate School, Tsinghua University
Xing Cheng: Tsinghua Shenzhen International Graduate School, Tsinghua University
Shaoke Guo: Tsinghua Shenzhen International Graduate School, Tsinghua University
Zhuo Han: Tsinghua Shenzhen International Graduate School, Tsinghua University
Tingzheng Hou: Tsinghua Shenzhen International Graduate School, Tsinghua University
Yidan Cao: Tsinghua Shenzhen International Graduate School, Tsinghua University
Ming Liu: Tsinghua Shenzhen International Graduate School, Tsinghua University
Wei Lv: Tsinghua Shenzhen International Graduate School, Tsinghua University
Yan-Bing He: Tsinghua Shenzhen International Graduate School, Tsinghua University
Feiyu Kang: Tsinghua Shenzhen International Graduate School, Tsinghua University

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Solid polymer electrolytes (SPEs) are considered as promising electrolytes for high-voltage lithium metal batteries. Whereas, the strong dipole-dipole interaction in polymer electrolytes limits the enhancement of the ionic conductivity. Here, we propose the 1,1,2,2-Tetrafluoroethyl-2,2,3,3-Tetrafluoropropylether (TTE) diluent to significantly regulate the dipole-dipole interaction in polymer-ionic solvate electrolytes (TPISEs). The TTE encapsulates ionic solvate to reduce the dipole-dipole interaction of ionic solvate with the polymer matrix, which promotes their homogeneous distribution, creating a continuous ion percolating network among the polymer matrix. The ion conductivity of TPISEs is therefore enhanced to 1.27×10−3 S cm−1 at 25 °C. Meanwhile, the TTE induces the ionic solvate to transform from contact ion pairs to aggregates, contributing to a stable lithium/electrolyte interface with exchange current density 190 times larger than that without TTE. The Li||LiNi0.8Co0.1Mn0.1O2 full cells exhibit good cycling stability from −30 °C to 60 °C. The practical pouch cells consisting of a thin Li metal foil (50 μm) and a high-areal-capacity positive electrode (3.58 mAh cm−2) achieve a high specific energy of 354.4 Wh·kg−1 and maintain 78.1% capacity after 450 cycles at 54 mA g−1 and 25 °C. This work provides a design strategy for SPEs beyond the bottleneck of ionic conductivity for practical solid-state batteries.

Date: 2025
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DOI: 10.1038/s41467-025-58689-3

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